The focused ion beam (FIB) technique was used to fabricate a nanothermocouple (with a 90 nm wide nanojunction) based on a metal–semiconductor (Pt–Si) structure, which showed a sensitivity up to 10 times larger (with Seebeck coefficient up to 140 µV/K) than typical metal–metal nanothermocouples. In contrast to the fabrication of nanothermocouples which requires a high-tech semiconductor manufacturing line with sophisticated fabrication techniques, environment, and advanced equipment, FIB systems are available in many research laboratories without the need for a high-tech environment, and the described processing is performed relatively quickly by a single operator. The linear response of the manufactured nanothermocouple enabled sensitive measurements even with small changes of temperature when heated with a stream of hot air. A nonlinear response of the nanothermocouple (up to 83.85 mV) was observed during the exposition to an argon-laser beam with a high optical power density (up to 17.4 Wcm−2), which was also used for the laser annealing of metal–semiconductor interfaces. The analysis of the results implies the application of such nanothermocouples, especially for the characterization of laser beams with nanometer spatial resolution. Improvements of the FIB processing should lead to an even higher Seebeck coefficient of the nanothermocouples; e.g., in case of the availability of other suitable metal sources (e.g., Cr).